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OH-Radical Oxidation of Lung Surfactant Protein B on Aqueous Surfaces.

ABSTRACT: Air pollutants generate reactive oxygen species on lung surfaces. Here we report how hydroxyl radicals (·OH) injected on the surface of water react with SP-B_1-25, a 25-residue polypeptide surrogate of human lung surfactant protein B. Our experiments consist of intersecting microjets of aqueous SP-B_1-25 solutions with O₃/O₂/H₂O/N₂(g) gas streams that are photolyzed into ·OH(g) in situ by 266 nm laser nanosecond pulses. Surface-sensitive mass spectrometry enables us to monitor the prompt (<10 μs) and simultaneous formation of primary O _n -containing products/intermediates (n≤5) triggered by the reaction of ·OH with interfacial SP-B_1-25. We found that O-atoms from both O₃ and ·OH are incorporated into the reactive cysteine Cys₈ and Cys₁₁ and tryptophan Trp₉ components of the hydrophobic N-terminus of SP-B_1-25 that lies at the topmost layers of the air-liquid interface. Remarkably, these processes are initiated by ·OH additions rather than by H-atom abstractions from S-H, C-H, or N-H groups. By increasing the hydrophilicity of the N-terminus region of SP-B_1-25, these transformations will impair its role as a surfactant.

SUBMITTER: Enami S

PROVIDER: S-EPMC6245955 | biostudies-literature | 2018

REPOSITORIES: biostudies-literature

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OH-Radical Oxidation of Lung Surfactant Protein B on Aqueous Surfaces.

Enami Shinichi S Colussi Agustín J AJ

Mass spectrometry (Tokyo, Japan) 20181121 2

Air pollutants generate reactive oxygen species on lung surfaces. Here we report how hydroxyl radicals (·OH) injected on the surface of water react with SP-B1-25, a 25-residue polypeptide surrogate of human lung surfactant protein B. Our experiments consist of intersecting microjets of aqueous SP-B1-25 solutions with O3/O2/H2O/N2(g) gas streams that are photolyzed into ·OH(g) in situ by 266 nm laser nanosecond pulses. Surfa ...[more]

PMID: 30533342

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Project description:C5- and C6- unsaturated oxygenated organic compounds emitted by plants under stress like cutting, freezing or drying, known as Green Leaf Volatiles (GLVs), may clear some of the existing uncertainties in secondary organic aerosol (SOA) budget. The transformations of GLVs are a potential source of SOA components through photo-oxidation processes occurring in the atmospheric aqueous phase. Here, we investigated the aqueous photo-oxidation products from three abundant GLVs (1-penten-3-ol, (Z)-2-hexen-1-ol, and (E)-2-hexen-1-al) induced by OH radicals, carried out in a photo-reactor under simulated solar conditions. The aqueous reaction samples were analyzed using advanced hyphenated mass spectrometry techniques: capillary gas chromatography mass spectrometry (c-GC-MS); and reversed-phase liquid chromatography high resolution mass spectrometry (LC-HRMS). Using carbonyl-targeted c-GC-MS analysis, we confirmed the presence of propionaldehyde, butyraldehyde, 1-penten-3-one, and 2-hexen-1-al in the reaction samples. The LC-HRMS analysis confirmed the presence of a new carbonyl product with the molecular formula C6H10O2, which probably bears the hydroxyhexenal or hydroxyhexenone structure. Density functional theory (DFT)-based quantum calculations were used to evaluate the experimental data and obtain insight into the formation mechanism and structures of the identified oxidation products via the addition and hydrogen-abstraction pathways. DFT calculations highlighted the importance of the hydrogen abstraction pathway leading to the new product C6H10O2. Atmospheric relevance of the identified products was evaluated using a set of physical property data like Henry's law constant (HLC) and vapor pressure (VP). The unknown product of molecular formula C6H10O2 has higher HLC and lower VP than the parent GLV and thus has potential to remain in the aqueous phase leading to possible aqueous SOA formation. Other observed carbonyl products are likely first stage oxidation products and precursors of aged SOA.

Dataset Information

OH-Radical Oxidation of Lung Surfactant Protein B on Aqueous Surfaces.

Publications

OH-Radical Oxidation of Lung Surfactant Protein B on Aqueous Surfaces.

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